An: Ab initio multiple cloning approach for the simulation of photoinduced dynamics in conjugated molecules

6Citations
Citations of this article
11Readers
Mendeley users who have this article in their library.

Abstract

We present a new implementation of the Ab Initio Multiple Cloning (AIMC) method, which is applied for non-adiabatic excited-state molecular dynamics simulations of photoinduced processes in conjugated molecules. Within our framework, the multidimensional wave-function is decomposed into a superposition of a number of Gaussian coherent states guided by Ehrenfest trajectories that are suited to clone and swap their electronic amplitudes throughout the simulation. New generalized cloning criteria are defined and tested. Because of sharp changes of the electronic states, which are common for conjugated polymers, the electronic parts of the Gaussian coherent states are represented in the Time Dependent Diabatic Basis (TDDB). The input to these simulations in terms of the excited-state energies, gradients and non-adiabatic couplings, is calculated on-the-fly using the Collective Electron Oscillator (CEO) approach. As a test case, we consider the photoinduced unidirectional electronic and vibrational energy transfer between two- and three-ring linear poly(phenylene ethynylene) units linked by meta-substitution. The effects of the cloning procedure on electronic and vibrational coherence, relaxation and unidirectional energy transfer between dendritic branches are discussed.

Cite

CITATION STYLE

APA

Freixas, V. M., Fernandez-Alberti, S., Makhov, D. V., Tretiak, S., & Shalashilin, D. (2018). An: Ab initio multiple cloning approach for the simulation of photoinduced dynamics in conjugated molecules. Physical Chemistry Chemical Physics, 20(26), 17762–17772. https://doi.org/10.1039/c8cp02321b

Register to see more suggestions

Mendeley helps you to discover research relevant for your work.

Already have an account?

Save time finding and organizing research with Mendeley

Sign up for free